Publications by David Mark Wilkins

Dissecting the hydrogen bond network of water: Charge transfer and nuclear quantum effects

Sylvie Roke, David Mark Wilkins, Mischa Samuel Flór

The molecular structure of water is dynamic, with intermolecular hydrogen (H) bond interactions being modified by both electronic charge transfer and nuclear quantum effects (NQEs). Electronic charge transfer and NQEs potentially change under acidic or bas ...

American Association for the Advancement of Science2024

Gaussian Process Regression for Materials and Molecules

Michele Ceriotti, David Mark Wilkins

We provide an introduction to Gaussian process regression (GPR) machinelearning methods in computational materials science and chemistry. The focus of the present review is on the regression of atomistic properties: in particular, on the construction of in ...

AMER CHEMICAL SOC2021

Inexpensive modeling of quantum dynamics using path integral generalized Langevin equation thermostats

Michele Ceriotti, Jinggang Lan, David Mark Wilkins, Venkat Kapil

The properties of molecules and materials containing light nuclei are affected by their quantum mechanical nature. Accurate modeling of these quantum nuclear effects requires computationally demanding path integral techniques. Considerable success has been ...

2020

Predicting molecular dipole moments by combining atomic partial charges and atomic dipoles

Michele Ceriotti, David Mark Wilkins, Max David Veit, Yang Yang

The molecular dipole moment (mu) is a central quantity in chemistry. It is essential in predicting infrared and sum-frequency generation spectra as well as induction and long-range electrostatic interactions. Furthermore, it can be extracted directly-via t ...

AMER INST PHYSICS2020

Correction to “Second-Harmonic Scattering as a Probe of Structural Correlations in Liquids”

Sylvie Roke, Michele Ceriotti, Gabriele Tocci, Chung-Wen Liang, David Mark Wilkins

2019

Determination and evaluation of the nonadditivity in wetting of molecularly heterogeneous surfaces

Francesco Stellacci, Quy Ong Khac, Sylvie Roke, Zhi Luo, Michele Ceriotti, Filip Kovacik, David Mark Wilkins, Halil Ibrahim Okur, Anna Murello

The interface between water and folded proteins is very complex. Proteins have "patchy" solvent-accessible areas composed of domains of varying hydrophobicity. The textbook understanding is that these domains contribute additively to interfacial properties ...

National Academy of Sciences2019

i-PI 2.0: A universal force engine for advanced molecular simulations

Anne-Clémence Corminboeuf, Riccardo Petraglia, Sébastien Pierre Bienvenue, Michele Ceriotti, Bingqing Cheng, David Mark Wilkins, Przemyslaw Juda, Benjamin Aaron Helfrecht, Venkat Kapil, Mariana Rossi Carvalho, Robert Horst Meissner, Alice Cuzzocrea, Gareth Aneurin Tribello, Wei Fang

Progress in the atomic-scale modeling of matter over the past decade has been tremendous. This progress has been brought about by improvements in methods for evaluating interatomic forces that work by either solving the electronic structure problem explici ...

ELSEVIER SCIENCE BV2019

Accurate molecular polarizabilities with coupled cluster theory and machine learning

Michele Ceriotti, David Mark Wilkins, Andrea Grisafi, Yang Yang

The molecular dipole polarizability describes the tendency of a molecule to change its dipole moment in response to an applied electric field. This quantity governs key intra- and intermolecular interactions, such as induction and dispersion; plays a vital ...

2019

Learning (from/about) the ground-state electron density

Anne-Clémence Corminboeuf, Alberto Fabrizio, Michele Ceriotti, David Mark Wilkins, Andrea Grisafi, Benjamin André René Meyer

AMER CHEMICAL SOC2019

Quantum mechanical static dipole polarizabilities in the QM7b and AlphaML showcase databases

Michele Ceriotti, David Mark Wilkins, Andrea Grisafi, Yang Yang

While density functional theory (DFT) is often an accurate and efficient methodology for evaluating molecular properties such as energies and multipole moments, this approach often yields larger errors for response properties such as the dipole polarizabil ...

2019

Transferable Machine-Learning Model of the Electron Density

Anne-Clémence Corminboeuf, Alberto Fabrizio, Michele Ceriotti, David Mark Wilkins, Andrea Grisafi, Benjamin André René Meyer

The electronic charge density plays a central role in determining the behavior of matter at the atomic scale, but its computational evaluation requires demanding electronic-structure calculations. We introduce an atom-centered, symmetry-adapted framework t ...

2019

Symmetry-Adapted Machine Learning for Tensorial Properties of Atomistic Systems

Michele Ceriotti, David Mark Wilkins, Andrea Grisafi

2018

Fast-forward Langevin dynamics with momentum flips

Michele Ceriotti, David Mark Wilkins, Mahdi Hijazi

2018

Jones-Ray effect reinterpreted: Surface tension minima of low ionic strength electrolyte solutions are caused by electric field induced water-water correlations

Yixing Chen, Sylvie Roke, David Mark Wilkins, Halil Ibrahim Okur

ACS2018

Comment on "Water- water correlations in electrolyte solutions probed by hyper-Rayleigh scattering" [J. Chem. Phys. 147, 214505 (2017)]

Yixing Chen, Sylvie Roke, Nathan Dupertuis, Michele Ceriotti, David Mark Wilkins, Halil Ibrahim Okur, Jan Dedic

AMER INST PHYSICS2018

The Molecular Mechanism of Nanodroplet Stability

Yixing Chen, Sylvie Roke, Evangelia Zdrali, David Mark Wilkins, Halil Ibrahim Okur

Mixtures of nano- and microscopic oil droplets in water have recently been rediscovered as miniature reaction vessels in microfluidic environments and are important constituents of many environmental systems, food, personal care, and medical products. The ...

Amer Chemical Soc2017

Solvent fluctuations and nuclear quantum effects modulate the molecular hyperpolarizability of water

Sylvie Roke, Michele Ceriotti, Gabriele Tocci, Chung-Wen Liang, David Mark Wilkins, Andrea Grisafi

Second-harmonic scattering (SHS) experiments provide a unique approach to probe noncentrosymmetric environments in aqueous media, from bulk solutions to interfaces, living cells, and tissue. A central assumption made in analyzing SHS experiments is that ea ...

Amer Physical Soc2017

Communication: Mean-field theory of water-water correlations in electrolyte solutions

Sylvie Roke, Michele Ceriotti, David Mark Wilkins

Long-range ion induced water-water correlations were recently observed in femtosecond elastic second harmonic scattering experiments of electrolyte solutions. To further the qualitative understanding of these correlations, we derive an analytical expressio ...

American Institute of Physics2017

Nuclear Quantum Effects in Water Reorientation and Hydrogen-Bond Dynamics

David Mark Wilkins

We combine classical and ring polymer molecular dynamics simulations with the molecular jump model to provide a molecular description of the nuclear quantum effects (NQEs) on water reorientation and hydrogen-bond dynamics in liquid H2O and D2O. We show tha ...

Amer Chemical Soc2017

Electrolytes induce long-range orientational order and free energy changes in the H-bond network of bulk water

Yixing Chen, Sylvie Roke, Nikolaos Gomopoulos, Carlos Alberto Macias Romero, Michele Ceriotti, Gabriele Tocci, Chung-Wen Liang, David Mark Wilkins, Halil Ibrahim Okur

Electrolytes interact with water in many ways: changing dipole orientation, inducing charge transfer, and distorting the hydrogen-bond network in the bulk and at interfaces. Numerous experiments and computations have detected short-range perturbations that ...

American Association for the Advancement of Science (AAAS)2016